Modified Activation-Relaxation Technique (ARTn) Method Tuned for Efficient Identification of Transition States in Surface Reactions.

Exploring potential energy surfaces (PES) is essential for unraveling the underlying mechanisms of chemical reactions and material properties. While the activation-relaxation technique (ARTn) is a state-of-the-art method for identifying saddle points on PES, it often faces challenges in complex energy landscapes, especially on surfaces. In this study, we introduce iso-ARTn, an enhanced ARTn method that incorporates constraints on an orthogonal hyperplane and employs an adaptive active volume. By leveraging a neural network potential (NNP) to conduct an exhaustive saddle point search on the Pt(111) surface with 0.3 monolayers of surface oxygen coverage, iso-ARTn achieves a success rate that is 8.2% higher than the original ARTn, with 40% fewer force calls. Moreover, this method effectively finds various saddle points without compromising the success rate. Combined with kinetic Monte Carlo simulations for event table construction, iso-ARTn with NNP demonstrates the capability to reveal structures consistent with experimental observations. This work signifies a substantial advancement in the investigation of PES, enhancing both the efficiency and breadth of saddle point searches.